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An environmentally benign three‐component Biginelli protocol for the one‐pot synthesis of substituted 3,4‐dihydropyrimidin‐2(1H)‐ones/thiones using an accessible, nontoxic, easy to handle, and recoverable macromolecular Lewis acidic catalyst is developed. N,N′‐methylene bis‐acrylamide‐cross‐linked poly(N‐vinyl‐2‐pyrrolidone) (MBA‐PVNP) as beads was used as a support for ferric chloride, resulting in a heterogeneous and reusable catalyst. The reusability test of the heterogenized version of ferric chloride, PNVP/FeCl3 ascertained that the obtained catalyst can be easily separated from the reaction mixture by filtration and reused several times with no great decline of activity.